Realization of Stable Ferromagnetic Order in Topological Insulator: Codoping Enhanced Magnetism in 4f Transition Metal Doped Bi2Se3

The realization of long range and insulating ferromagnetic states in topological insulator (TI) has been a pressing issue since its discovery. Only recently, such state was achieved in Cr-doped Bi2-xSbxTe3, leading to the discovery of quantum anomalous Hall effect (QAHE). However, the effect is only observed at extremely low temperatures mainly due to the limited magnetism. To fully understand the mechanism of the ferromagnetic ordering whereby improving the ferromagnetism, we investigated 4f transition metal-doped Bi2Se3, using density-functional-theory approaches. We found that Eu and Sm prefer the Bi substitutional sites with large magnetic moments to ensure stable long-range ferromagnetic states. Additionally, codoping can be a novel strategy to preserve the insulating property of the host material as well as improving the incorporation of magnetic dopants. Our findings thus offer the critical step in facilitating the realization of QAHE in TI systems.